Pd@C2N单原子催化剂用于HCOOH分解制氢的第一性原理研究

First-principle study of hydrogen production from HCOOH dehydrogenation on Pd@C2N single-atom catalyst

用于HCOOH分解制氢的贵金属催化剂存在着反应选择性差和资源稀缺等问题.单原子催化可以有效改善催化剂性能并降低成本,C2N作为一种新型二维材料可为过渡金属原子提供良好的结合位点.本文利用密度泛函理论,设计了Pd@C2N单原子催化剂,研究了HCOOH在Pd@C2N表面上的吸附和分解制氢反应机理.结果表明,HCOOH可在Pd原子顶位吸附,并在C2N表面N原子的协同作用下通过甲酸盐路径生成氢气.通过比较,Pd@C2N具有比Pd(111)表面更好的催化反应活性与选择性.

The poor selectivity and resource scarcity restrict the application of noble metal catalysts in hydrogen production from HCOOH dehydrogenation reaction.Single-atom catalysis(SAC)can effectively improve catalyst performance and reduce cost.As a novel two-dimensional material,C2N can provide ideal binding sites for transition metal atoms.In this work,using the density functional theory(DFT),we designed the Pd@C2N single-atom catalyst and studied the HCOOH adsorption and dehydrogenation mechanism on Pd@C2N surface.The results show that HCOOH can adsorb at the top site of Pd atom.The dehydrogenation reaction prefers the formate path to generate hydrogen under the synergistic effect of N atom on C2N.Pd@C2N also has the better catalytic activity and selectivity than the Pd(111)surface.